DataVXAdvanced MaterialsPaper
journal article·2022-09Open access

Tackling Disorder in γ‐Ga2O3

Laura E. Ratcliff, Takayoshi Oshima, Felix Nippert, Benjamin M. Janzen, Elias Kluth, Rüdiger Goldhahn, Martin Feneberg, Piero Mazzolini, Oliver Bierwagen, Charlotte Wouters, Musbah Nofal, Martin Albrecht, Jack E. N. Swallow, Leanne A. H. Jones, Pardeep K. Thakur, Tien‐Lin Lee, Curran Kalha, Christoph Schlueter, Tim D. Veal, Joel B. Varley, Markus R. Wagner, Anna Regoutz

Advanced Materials· Volume 34· Issue 37
Publisher pageOpen full text
Source abstract

Abstract

Abstract Ga2O3 and its polymorphs are attracting increasing attention. The rich structural space of polymorphic oxide systems such as Ga2O3 offers potential for electronic structure engineering, which is of particular interest for a range of applications, such as power electronics. γ‐Ga2O3 presents a particular challenge across synthesis, characterization, and theory due to its inherent disorder and resulting complex structure–electronic‐structure relationship. Here, density functional theory is used in combination with a machine‐learning approach to screen nearly one million potential structures, thereby developing a robust atomistic model of the γ‐phase. Theoretical results are compared with surface and bulk sensitive soft and hard X‐ray photoelectron spectroscopy, X‐ray absorption spectroscopy, spectroscopic ellipsometry, and photoluminescence excitation spectroscopy experiments representative of the occupied and unoccupied states of γ‐Ga2O3. The first onset of strong absorption at room temperature is found at 5.1 eV from spectroscopic ellipsometry, which agrees well with the excitation maximum at 5.17 eV obtained by photoluminescence excitation spectroscopy, where the latter shifts to 5.33 eV at 5 K. This work presents a leap forward in the treatment of complex, disordered oxides and is a crucial step toward exploring how their electronic structure can be understood in terms of local coordination and overall structure.
Source: crossref · Quality: baseline

Research context

OpenAlex topics: Ga2O3 and related materials · Electronic and Structural Properties of Oxides · Advanced Photocatalysis Techniques

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Materials Imperial College London London SW7 2AZ UK

Center for Computational Chemistry School of Chemistry University of Bristol Bristol BS8 1TS UK

Department of Electrical and Electronic Engineering Saga University Saga 840‐8502 Japan

Technische Universität Berlin Institute of Solid State Physics Hardenbergstrasse 36 10623 Berlin Germany

Institut für Physik Otto‐von‐Guericke‐Universität Magdeburg Universitätsplatz 2 39106 Magdeburg Germany

Paul‐Drude‐Institut für Festkörperelektronik Leibniz‐Institut im Forschungsverbund Berlin e.V. Hausvogteiplatz 5‐7 10117 Berlin Germany

Leibniz‐Institut für Kristallzüchtung Max‐Born‐Str. 2 12489 Berlin Germany

Department of Materials University of Oxford Parks Road Oxford OX1 3PH UK

Stephenson Institute for Renewable Energy and Department of Physics University of Liverpool Liverpool L69 7ZF UK

Diamond Light Source Ltd. Diamond House Harwell Science and Innovation Campus Didcot OX11 0DE UK

Department of Chemistry University College London 20 Gordon Street London WC1H 0AJ UK

Deutsches Elektronen‐Synchrotron DESY Notkestrasse 85 22607 Hamburg Germany

Lawrence Livermore National Laboratory Livermore CA 94550 USA

Funding

Engineering and Physical Sciences Research Council · Thomas Young Centre · Deutsche Forschungsgemeinschaft · Lawrence Livermore National Laboratory

References (57)

Show source-provided references
1. 10.1063/1.500694110.1063/1.5006941 ↗
2. 10.1002/adma.20200623010.1002/adma.202006230 ↗
3. 10.1016/j.mtphys.2019.10015710.1016/j.mtphys.2019.100157 ↗
4. 10.1002/adma.20140204710.1002/adma.201402047 ↗
5. 10.1088/1361-6463/abbb4510.1088/1361-6463/abbb45 ↗
6. 10.1016/j.apcatb.2019.11824710.1016/j.apcatb.2019.118247 ↗
7. 10.1088/0268-1242/31/3/03400110.1088/0268-1242/31/3/034001 ↗
8. 10.1186/s11671-018-2712-110.1186/s11671-018-2712-1 ↗
9. 10.1002/chem.20120335910.1002/chem.201203359 ↗
10. 10.1002/ange.1940053111610.1002/ange.19400531116 ↗
11. 10.1021/ja01123a03910.1021/ja01123a039 ↗
12. 10.1007/BF0059949010.1007/BF00599490 ↗
13. 10.1021/jp503380610.1021/jp5033806 ↗
14. 10.1103/PhysRev.136.B86410.1103/PhysRev.136.B864 ↗
15. 10.1103/PhysRev.140.A113310.1103/PhysRev.140.A1133 ↗
16. 10.1088/0953-8984/19/34/34621110.1088/0953-8984/19/34/346211 ↗
17. 10.1063/1.477036310.1063/1.4770363 ↗
18. 10.1103/PhysRevB.65.01210110.1103/PhysRevB.65.012101 ↗
19. 10.1103/PhysRevB.70.12540210.1103/PhysRevB.70.125402 ↗
20. 10.1021/jp057341p10.1021/jp057341p ↗
21. 10.1002/aelm.20200011910.1002/aelm.202000119 ↗
22. 10.1063/5.001210310.1063/5.0012103 ↗
23. 10.1103/PhysRevB.71.22411510.1103/PhysRevB.71.224115 ↗
24. 10.1021/acs.chemmater.0c0246510.1021/acs.chemmater.0c02465 ↗
25. 10.1063/1.349930610.1063/1.3499306 ↗
26. 10.1063/1.493470510.1063/1.4934705 ↗
27. E.Kluth P.Ning J.Grümbel A.Karg M.Eickhoff R.Goldhahn M.Feneberg unpublished.
28. 10.1103/PhysRevMaterials.2.04460110.1103/PhysRevMaterials.2.044601 ↗
29. 10.1063/1.10472310.1063/1.104723 ↗
30. 10.1002/1521-3951(199703)200:1<155::AID-PSSB155>3.0.CO;2-310.1002/1521-3951(199703)200:1<155::AID-PSSB155>3.0.CO;2-3 ↗
31. 10.1103/PhysRevB.93.11520410.1103/PhysRevB.93.115204 ↗
32. 10.1063/1.508432410.1063/1.5084324 ↗
33. 10.1016/j.cap.2012.05.03810.1016/j.cap.2012.05.038 ↗
34. 10.1103/PhysRevLett.77.386510.1103/PhysRevLett.77.3865 ↗
35. 10.1063/5.000479210.1063/5.0004792 ↗
36. 10.1103/PhysRevB.54.170310.1103/PhysRevB.54.1703 ↗
37. 10.1103/PhysRevB.58.364110.1103/PhysRevB.58.3641 ↗
38. 10.1063/1.479326010.1063/1.4793260 ↗
39. 10.1524/zkri.220.5.567.6507510.1524/zkri.220.5.567.65075 ↗
40. 10.1103/PhysRevB.13.518810.1103/PhysRevB.13.5188 ↗
41. 10.1016/j.cpc.2014.02.01310.1016/j.cpc.2014.02.013 ↗
42. J. H.Scofield Theoretical Photoionization Cross Sections from 1 to 1500 keV Technical report U.S. Atomic Energy Commission Divison of Technical Information Extension 1973 https://www.osti.gov/biblio/4545040/(accessed: May 2022).10.2172/4545040 ↗
43. C.Kalha N. K.Fernando A.Regoutz Digitisation of Scofield Photoionisation Cross Section tabulated data2020 https://figshare.com/articles/dataset/Digitisation_of_Scofield_Photoionisation_Cross_Section_Tabulated_Data/12967079(accessed: May 2022).
44. 10.21105/joss.0077310.21105/joss.00773 ↗
45. 10.1107/S010827019501640410.1107/S0108270195016404 ↗
46. 10.1021/acs.chemrev.1c0002110.1021/acs.chemrev.1c00021 ↗
47. 10.1021/acs.chemrev.1c0010710.1021/acs.chemrev.1c00107 ↗
48. Pedregosa F. · J. Mach. Learn. Res. · 2011 · 12 · 2825
49. 10.1063/5.005854110.1063/5.0058541 ↗
50. 10.7567/APEX.10.05110410.7567/APEX.10.051104 ↗
51. 10.7567/1347-4065/ab219f10.7567/1347-4065/ab219f ↗
52. 10.7567/1882-0786/ab219610.7567/1882-0786/ab2196 ↗
53. 10.1080/08940886.2018.148365310.1080/08940886.2018.1483653 ↗
54. 10.1063/1.508461110.1063/1.5084611 ↗
55. 10.1002/andp.1935416070510.1002/andp.19354160705 ↗
56. 10.1016/j.tsf.2013.11.14110.1016/j.tsf.2013.11.141 ↗
57. 10.1107/S002188981103897010.1107/S0021889811038970 ↗